Graphene oxide (GO) nanosheets are prepared by oxidation of graphite followed by sonication exfoliation. FTIR and AFM results indicate that the GO nanosheets have a thickness of about 6 nm, and that the GO surface is covered with oxygenated groups (–OH, –O–, –COOH and –SO₃H). Hardened cement pastes containing different proportions of the GO nanosheets are prepared, and it is found that the GO formed both flower-like and polyhedron-like crystals, with these effects increasing as the GO content increases from 0.01% to 0.06% by weight of the cement. The compressive strength and toughness of the corresponding hardened cement paste are found to be markedly increased compared to a control sample. The results suggest that the GO nanosheets can control the crystalline form and assembly of the cement hydration products. A formation mechanism for regular hydration crystals is proposed, based on the experimental results. This research indicates significant potential for the practical application of GO nanosheets in the preparation of cement-based materials of high strength and durability.

The main problem with cement composites is that they have structural defects, including cracks, holes, and a disordered morphology, which significantly affects their strength and durability. Therefore, the construction of cement composites with defect-free structures and high strength and long durability is an important research topic. Here, by controlling the size and chemical groups of graphene oxide nanosheets (GONs) used for doping, we were able to control the entire cement matrix to form an ordered microstructure consisting of polyhedron-like crystals and exhibit flower-like patterns. The cracks and holes in the cement matrix just about vanished. The compressive and flexural strengths as well as the parameters for the durability assessment of the corresponding cement composites obviously improved compared with the control samples. Thus, the formation mechanism of the cement matrix with the ordered microstructure is proposed, and a proper explanation is given to regulation action.

Original graphene oxide (GO) nanosheets were prepared using the Hummers method and found to easily aggregate in aqueous and cement composites. Using carboxymethyl chitosan (CCS) as a dispersant, few-layered GO nanosheets (1–2 layers) were obtained by forming CCS/GO intercalation composites. The testing results indicated that the few-layered GO nanosheets could uniformly spread, both in aqueous and cement composites. The cement composites were prepared with GO dosages of 0.03%, 0.05% and 0.07% and we found that they had a compact microstructure in the whole volume. A special feature was determined, namely that the microstructures consisted of regular-shaped crystals created by self-crosslinking. The X-ray diffraction (XRD) results indicated that there was a higher number of cement hydration crystals in GO/cement composites. Meanwhile, we also found that partially-amorphous Calcium-Silicate-Hydrate (C-S-H) gel turned into monoclinic crystals. At 28 days, the GO/cement composites reached the maximum compressive and flexural strengths at a 0.05% dosage. These strengths were 176.64 and 31.67 MPa and, compared with control samples, their increased ratios were 64.87% and 149.73%, respectively. Durability parameters, such as penetration, freeze-thaw, carbonation, drying-shrinkage value and pore structure, showed marked improvement. The results indicated that it is possible to obtain cement composites with a compact microstructure and with high performances by introducing CCS/GO intercalation composites.